EP0902754B1 - Method for inducing hydrogen desorption from a metal hydride - Google Patents

Method for inducing hydrogen desorption from a metal hydride Download PDF

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Publication number
EP0902754B1
EP0902754B1 EP97920469A EP97920469A EP0902754B1 EP 0902754 B1 EP0902754 B1 EP 0902754B1 EP 97920469 A EP97920469 A EP 97920469A EP 97920469 A EP97920469 A EP 97920469A EP 0902754 B1 EP0902754 B1 EP 0902754B1
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EP
European Patent Office
Prior art keywords
desorption
metal hydride
hydrogen
energy
hydride
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Lifetime
Application number
EP97920469A
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German (de)
French (fr)
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EP0902754A1 (en
Inventor
Alicja Zaluska
Leszek Zaluski
John Strom-Olsen
Robert Schulz
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Hydro Quebec
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McGill University
Hydro Quebec
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Application filed by McGill University, Hydro Quebec filed Critical McGill University
Priority to EP03014112A priority Critical patent/EP1382566A1/en
Publication of EP0902754A1 publication Critical patent/EP0902754A1/en
Application granted granted Critical
Publication of EP0902754B1 publication Critical patent/EP0902754B1/en
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    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/0005—Reversible uptake of hydrogen by an appropriate medium, i.e. based on physical or chemical sorption phenomena or on reversible chemical reactions, e.g. for hydrogen storage purposes ; Reversible gettering of hydrogen; Reversible uptake of hydrogen by electrodes
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/04—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of inorganic compounds, e.g. ammonia
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B6/00—Hydrides of metals including fully or partially hydrided metals, alloys or intermetallic compounds ; Compounds containing at least one metal-hydrogen bond, e.g. (GeH3)2S, SiH GeH; Monoborane or diborane; Addition complexes thereof
    • C01B6/04—Hydrides of alkali metals, alkaline earth metals, beryllium or magnesium; Addition complexes thereof
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B6/00—Hydrides of metals including fully or partially hydrided metals, alloys or intermetallic compounds ; Compounds containing at least one metal-hydrogen bond, e.g. (GeH3)2S, SiH GeH; Monoborane or diborane; Addition complexes thereof
    • C01B6/24—Hydrides containing at least two metals; Addition complexes thereof
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C11/00—Use of gas-solvents or gas-sorbents in vessels
    • F17C11/005—Use of gas-solvents or gas-sorbents in vessels for hydrogen
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/32—Hydrogen storage
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis

Definitions

  • the present invention relates to a method for inducing desorption of hydrogen from a metal hydride containing the same, in which a non-thermal energy source is used to induce such desorption.
  • Metal hydrides are potentially ideal candidates for hydrogen storage and transportation. As hydrogen carriers, they provide high hydrogen storage capacities (up to for example 7.6 wt. % in Mg 2 H 2 ) and full safety. The safety is provided by endothermic reaction of hydrogen release, which excludes spontaneous (explosive) or uncontrolled reaction.
  • Metal hydrides are advantageous in that they can be handled and stored at ambient temperature without any atmosphere or pressure requirements. Such makes them economically favorable by elimination of cryogenic equipment necessary to use with liquid hydrogen or activated charcoal.
  • GB-A-1568374 and GB-A-2 164 637 disclose metallic hydride hydrogen storages and respectively process for the supply of hydrogen from a metallic hydride material.
  • Metal hydrides are also very stable. Such is advantageous from a safety and economical point of view. However, because of their stability, most of the metal hydrides require elevated temperatures to initiate desorption.
  • metal hydrides having a high stability are MgH 2 or Mg 2 NiH 4 . They exhibit excellent hydrogen storage potential - with large hydrogen storage capacity (7.65 wt. % for MgH 2 or 3.6 wt. % for Mg 2 NiH 4 ), low cost of the material and easy handling. However, desorption of hydrogen from these hydrides with reasonable kinetics requires heating to high temperatures: 350 - 400°C for MgH 2 and 330 - 360°C for Mg 2 NiH 4 .
  • the object of the present invention is to provide an alternative approach to facilitate desorption of hydrogen from a high temperature metal hydride.
  • the invention is based on the discovery that, instead of using a conventional heat source, use can be made of a non-thermal energy source to initiate hydrogen release and thus to induce hydrogen desorption.
  • non-thermal energy sources does not necessary exclude energy sources where heat is produced, like electric energy where heat is produced by Joule effect.
  • this expression is exclusively used to exclude “conventional” heat sources such as gas or oil burners where heat is produced and transferred mainly by convection to the metal hydrides.
  • the present invention as broadly claimed hereinafter, is directed to a method for inducing desorption of hydrogen from a metal hydride by applying thereto sufficient energy to induce hydrogen desorption by endothermic reaction, wherein the energy that is so applied is non-thermal and consists of mechanical energy.
  • the invention is based on the discovery that instead of using a heat source as it has been done so far, use can be made of a non-thermal energy source to induce hydrogen desorption from a metal hydride.
  • This energy is applied directly on the metal hydride.
  • One way to apply the energy directly to the metal hydride consists in introducing an accumulating energy in the hydride to cause desorption by mechanical energy (in the form of strain and defects).
  • desorption is much easier than when the hydride is activated by heat. Moreover, after mechanical pretreatment, the desorption temperature is significantly reduced.
  • the method of inducing hydrogen desorption from a metal hydride consists of applying mechanical energy by ball milling to a powder of the metal hydride (which is the usual form of metal hydride). It is well established that ball milling is capable of generating a sufficient amount of mechanical energy to cause formation of various compounds (nitrides, borides,) or alloys (mechanical alloying). In the present case, ball milling can be used either to decompose the metal hydride and release hydrogen, or to accumulate so much strain and defects in the hydride that further heat-activated desorption is facilitated. Temperature of desorption of metal hydrides treated mechanically may be then reduced by 100 - 200°C, which is of great significance for practical application.
  • the method according to the invention may be used for inducing hydrogen desorption in disposable hydrogen storage tanks (for camping units or similar use).
  • Fig. 1 are differential scanning calorimetry (DSC) curves of a Mg-based hydride as prepared (a) and after 2, 7 and 9 minutes of ball milling (curves (b), (c) and (d), respectively).
  • DSC differential scanning calorimetry
  • a Mg-based hydride was submitted to a mechanical pretreatment before desorption.
  • it In the as-prepared state, it exhibited a high temperature of desorption equal to about 400°C, when measured by differential scanning calorimetry (DSC) at continuous heating with heating rate of 40 K/min (see Fig. 2, curve a).
  • DSC differential scanning calorimetry
  • Ball milling in a SPEX® mill caused a decrease in the desorption temperature due to an accumulation of mechanical energy in the form of strain and defects.
  • Curves b, c and d represent effects of ball milling of the hydride for 2, 7, 9 min., respectively.
  • the temperature of desorption was decreased by 200°C in the last case (see Fig. 2).

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Inorganic Chemistry (AREA)
  • Combustion & Propulsion (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Geology (AREA)
  • General Life Sciences & Earth Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Hydrogen, Water And Hydrids (AREA)

Description

BACKGROUND OF THE INVENTION a) Field of the invention
The present invention relates to a method for inducing desorption of hydrogen from a metal hydride containing the same, in which a non-thermal energy source is used to induce such desorption.
b) Brief description of the prior art
Metal hydrides are potentially ideal candidates for hydrogen storage and transportation. As hydrogen carriers, they provide high hydrogen storage capacities (up to for example 7.6 wt. % in Mg2H2) and full safety. The safety is provided by endothermic reaction of hydrogen release, which excludes spontaneous (explosive) or uncontrolled reaction.
Metal hydrides are advantageous in that they can be handled and stored at ambient temperature without any atmosphere or pressure requirements. Such makes them economically favorable by elimination of cryogenic equipment necessary to use with liquid hydrogen or activated charcoal. GB-A-1568374 and GB-A-2 164 637 disclose metallic hydride hydrogen storages and respectively process for the supply of hydrogen from a metallic hydride material.
Metal hydrides are also very stable. Such is advantageous from a safety and economical point of view. However, because of their stability, most of the metal hydrides require elevated temperatures to initiate desorption.
Examples of metal hydrides having a high stability are MgH2 or Mg2NiH4. They exhibit excellent hydrogen storage potential - with large hydrogen storage capacity (7.65 wt. % for MgH2 or 3.6 wt. % for Mg2NiH4), low cost of the material and easy handling. However, desorption of hydrogen from these hydrides with reasonable kinetics requires heating to high temperatures: 350 - 400°C for MgH2 and 330 - 360°C for Mg2NiH4.
For many applications, heating to such temperatures is disadvantageous. Indeed, it increases technical problems of hydrogen recovery and reduces effectiveness of the devices.
To solve this problem, it has already been suggested to reduce the stability of high temperature metal hydrides. Such may be obtained by alloying the metal hydrides with other elements. However, stability reduction occurs at the expense of the total hydrogen capacity.
OBJECT AND SUMMARY OF THE INVENTION
The object of the present invention is to provide an alternative approach to facilitate desorption of hydrogen from a high temperature metal hydride.
More particularly, the invention is based on the discovery that, instead of using a conventional heat source, use can be made of a non-thermal energy source to initiate hydrogen release and thus to induce hydrogen desorption.
The expression "non-thermal energy sources" as used in the present specification and claims does not necessary exclude energy sources where heat is produced, like electric energy where heat is produced by Joule effect. As a matter of fact, this expression is exclusively used to exclude "conventional" heat sources such as gas or oil burners where heat is produced and transferred mainly by convection to the metal hydrides.
Thus, the present invention as broadly claimed hereinafter, is directed to a method for inducing desorption of hydrogen from a metal hydride by applying thereto sufficient energy to induce hydrogen desorption by endothermic reaction, wherein the energy that is so applied is non-thermal and consists of mechanical energy.
The invention and its advantages will be better understood upon reading the following, non-restrictive description and examples.
DETAILED DESCRIPTION OF THE INVENTION
As aforesaid, the invention is based on the discovery that instead of using a heat source as it has been done so far, use can be made of a non-thermal energy source to induce hydrogen desorption from a metal hydride.
Thus, instead of using heat energy to raise the temperature of the environment of the hydride in order to induce the endothermal reaction of desorption of hydrogen from the same, energy is supplied to the hydride either instrinsically and on a local scale.
This energy is applied directly on the metal hydride. One way to apply the energy directly to the metal hydride consists in introducing an accumulating energy in the hydride to cause desorption by mechanical energy (in the form of strain and defects).
In this particular case, desorption is much easier than when the hydride is activated by heat. Moreover, after mechanical pretreatment, the desorption temperature is significantly reduced.
4. Mechanical energy
The method of inducing hydrogen desorption from a metal hydride consists of applying mechanical energy by ball milling to a powder of the metal hydride (which is the usual form of metal hydride). It is well established that ball milling is capable of generating a sufficient amount of mechanical energy to cause formation of various compounds (nitrides, borides,) or alloys (mechanical alloying). In the present case, ball milling can be used either to decompose the metal hydride and release hydrogen, or to accumulate so much strain and defects in the hydride that further heat-activated desorption is facilitated. Temperature of desorption of metal hydrides treated mechanically may be then reduced by 100 - 200°C, which is of great significance for practical application.
Mechanical energy affects the structure of metal hydride. In such a case, the method according to the invention may be used for inducing hydrogen desorption in disposable hydrogen storage tanks (for camping units or similar use).
BRIEF DESCRIPTION OF THE DRAWING
Fig. 1 are differential scanning calorimetry (DSC) curves of a Mg-based hydride as prepared (a) and after 2, 7 and 9 minutes of ball milling (curves (b), (c) and (d), respectively).
EXAMPLE 1 - mechanical energy
A Mg-based hydride was submitted to a mechanical pretreatment before desorption. In the as-prepared state, it exhibited a high temperature of desorption equal to about 400°C, when measured by differential scanning calorimetry (DSC) at continuous heating with heating rate of 40 K/min (see Fig. 2, curve a). Ball milling in a SPEX® mill caused a decrease in the desorption temperature due to an accumulation of mechanical energy in the form of strain and defects. Curves b, c and d represent effects of ball milling of the hydride for 2, 7, 9 min., respectively. The temperature of desorption was decreased by 200°C in the last case (see Fig. 2).

Claims (3)

  1. A method for inducing desorption of hydrogen from a metal hydride wherein sufficient energy is applied onto said metal hydride to induce hydrogen desorption by endothermic reaction, characterized in that:
    the energy that is so applied consists of mechanical energy;
    and said mechanical energy is applied directly to the metal hydride by subjecting said metal hydride to a high energy mechanical grinding.
  2. The method of claim 1, characterized in that the mechanical energy is used exclusively to induce the hydrogen desorption and the so-induced hydrogen desorption is then completed by thermal heating.
  3. The method according to anyone of claims 1 to 2, according to which the metal hydride is selected from the group consisting of MgH2 and Mg2NiH4.
EP97920469A 1996-05-13 1997-05-13 Method for inducing hydrogen desorption from a metal hydride Expired - Lifetime EP0902754B1 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
EP03014112A EP1382566A1 (en) 1996-05-13 1997-05-13 Method for inducing hydrogen desorption from a metal hydride

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
US645352 1996-05-13
US08/645,352 US5882623A (en) 1996-05-13 1996-05-13 Method for inducing hydrogen desorption from a metal hydride
PCT/CA1997/000324 WO1997043206A1 (en) 1996-05-13 1997-05-13 Method for inducing hydrogen desorption from a metal hydride

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EP0902754A1 EP0902754A1 (en) 1999-03-24
EP0902754B1 true EP0902754B1 (en) 2003-08-06

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EP03014112A Withdrawn EP1382566A1 (en) 1996-05-13 1997-05-13 Method for inducing hydrogen desorption from a metal hydride

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US (2) US5882623A (en)
EP (2) EP0902754B1 (en)
JP (1) JP2000515107A (en)
CN (1) CN1094895C (en)
CA (1) CA2254858C (en)
DE (1) DE69723977T2 (en)
WO (1) WO1997043206A1 (en)

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Publication number Publication date
DE69723977T2 (en) 2004-07-29
US6080381A (en) 2000-06-27
WO1997043206A1 (en) 1997-11-20
EP0902754A1 (en) 1999-03-24
JP2000515107A (en) 2000-11-14
CA2254858C (en) 2002-07-30
CA2254858A1 (en) 1997-11-20
CN1222894A (en) 1999-07-14
DE69723977D1 (en) 2003-09-11
CN1094895C (en) 2002-11-27
US5882623A (en) 1999-03-16
EP1382566A1 (en) 2004-01-21

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